首页|Regulating *COOH intermediate via amino alkylation engineering for exceptionally effective photocatalytic CO2 reduction

Regulating *COOH intermediate via amino alkylation engineering for exceptionally effective photocatalytic CO2 reduction

扫码查看
原文链接
  • NETL
  • NSTL
  • 万方数据
Photocatalytic reduction of CO2 into fuel represents a promising approach for achieving carbon neutrality,while realizing high selectivity in this process is challenging due to uncontrollable reaction intermediate and retarded desorption of target products.Engineering the interface microenvironment of catalysts has been proposed as a strategy to exert a significant influence on reaction outcomes,yet it remains a signif-icant challenge.In this study,amino alkylation was successfully integrated into the melem unit of poly-meric carbon nitrides(PCN),which could efficiently drive the photocatalytic CO2 reduction.Experimental characterization and theoretical calculations revealed that the introduction of amino alkylation lowers the energy barrier for CO2 reduction into*COOH intermediate,transforming the adsorption of*COOH intermediate from the endothermic to an exothermic process.Notably,the as-prepared materials demon-strated outstanding performance in photocatalytic CO2 reduction,yielding CO at a rate of 152.8 μmol h-1 with a high selectivity of 95.4％and a quantum efficiency of 6.6％.

Polymeric carbon nitrideRegulate intermediatePhotocatalytic CO2 reductionAmino alkylation*COOH adsorption

Chengcheng Chen、Qiaoyu Zhang、Fangting Liu、Zhengguo Zhang、Qiong Liu、Xiaoming Fang

展开 >

Key Laboratory of Enhanced Heat Transfer and Energy Conservation,The Ministry of Education,School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640,Guangdong,China

Guangdong Engineering Technology Research Center of Efficient Heat Storage and Application,South China University of Technology,Guangzhou 510640,Guangdong,China

Guangdong Provincial Key Laboratory of Chemical Measurement and Emergency Test Technology(China),Institute of Analysis,Guangdong Academy of Sciences(China National Analytical Center,Guangzhou),Guangzhou 510070,Guangdong,China

Guangdong Provincial Key Laboratory of Fuel Cell Technology,South China University of Technology,Guangzhou 510640,Guangdong,China

展开 >

National Natural Science Foundation of ChinaGuangdong Basic and Applied Basic Research FoundationScience and Technology Program of GuangzhouGDAS'Project of Science and Technology Development

223090322022A15150117372023A04J13952021GDASYL-20210102010

2024

10.1016/j.jechem.2024.01.030

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.92(5)